The　noble　metal　catalysts　represented　by　Ru-　and　Ir-based　catalysts　and　their　oxides　have　excellent　OER　properties,　but　their　limited　earth　reserves　and　high　prices　have　severely　limited　the　large-scale　commercial　application　of　noble　metal　catalysts.　Nickel-iron　hydroxide　(Ni/Fe-LDHs)　is　considered　to　be　a　promising　non-precious　metal　OER　electrocatalyst　due　to　its　special　layered　structure　and　adjustable　composition.　Nevertheless,　the　edge　sites　serve　as　the　primary　active　centers　of　Ni/Fe-LDHs,　and　the　formation　of　the　highly　oxidized　catalytic　phase　is　impeded　by　the　closely　packed　substrate.　Therefore,　activation　of　these　substrates　is　particularly　important　for　further　enhancing　the　catalytic　activity　of　Ni/Fe-LDHs.　An　effective　strategy　for　addressing　this　issue　is　to　replace　two-dimensional　sheets　with　three-dimensional　materials.　In　this　study,　a　simple,　inexpensive,　and　self-assembly　strategy　was　developed　for　the　large-scale　preparation　of　Ni/Fe-LDHs　under　hydrothermal　conditions.　The　fabrication　mechanism　involves　a　stepwise　and　orderly　process　where　LDH　nanosheets　gradually　grow　into　nanopetals　before　assembling　into　flower-like　microspheres,　based　on　a　systematic　investigation　of　the　zeolite　4A　(ZA)　feeding　ratio.　Zeolite　plays　the　role　of　a　template　agent　in　the　growth　of　composite　materials.　The　specific　surface　area　of　the　Ni/Fe-LDHs/0.3　mg　ZA　composite　material　(336.0　m2/g)　is　increased　by　more　than　three　times　compared　that　with　pure　Ni/Fe-LDHs　(96.53　m2/g).　Owing　to　their　large　specific　surface　area,　ultrathin　structure,　and　the　synergistic　effects　of　the　Ni/Fe-LDHs/ZA　composite,　these　Ni/Fe-LDHs/ZA　microspheres　exhibit　excellent　electrochemical　performance.　The　Cdl　value,　overpotential,　and　OER　activity　of　Ni/Fe-LDHs/ZA　composites　were　also　enhanced　compared　with　pure　Ni/Fe-LDHs.　©　2025　Elsevier　Inc.